We present evaluations of the interaction of 20 to 100 MeV neutrons with calcium and phosphorus, which follows on from our previous work on carbon, nitrogen, and oxygen [l, 21. Our aim is to accurately represent integrated cross sections, inclusive emission spectra, and kerma factors, in a data library which can be used in radiation transport calculations. We apply the GNASH nuclear model code, which includes Hauser-Feshbach, preequilibrium, and direct reaction mechanisms, and use experimental measurements to optimize the calculations. Total, elastic, and nonelastic cross sections, angle-energy correlated emission spectra for light ejectiles with A 5 4 and gamma-rays, and average energy depositions, are determined. The expected accuracy of the calculated cross sections and kerma factors is discussed.